High catalytic activity for CO oxidation on single Fe atom stabilized in graphene vacancies

Tang, Yanan; Zhou, Jincheng; Shen, Zigang; Chen, Weiguang; Li, Chenggang; Dai, Xianqi

doi:10.1039/c6ra14476d

Cited by 65 publications

(28 citation statements)

References 93 publications

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“…Furthermore, as mentioned above divacancy is commonly present in graphene obtained through chemical synthesis. However, only the catalytic activity of Fe-decorated DV graphene has been studied (Tang et al, 2016 ; Liu et al, 2017 ). Therefore, further research about the catalytic performance of DV graphene decorated with metal atom for CO oxidation is needed.…”

Section: Introductionmentioning

confidence: 99%

“…In general, the reaction energy barriers are proportional to the adsorption energy of adsorbed molecules on supported catalyst (Gong et al, 2004 ), indicating that the adsorption energy of adsorbed CO and O 2 molecules could be a benchmark for the catalytic performance of graphene for CO oxidation. In addition, a larger adsorption energy for O 2 molecule than that of CO is desired during the CO oxidation progress, because the preferential adsorption of CO will block the active sites and prevent the continuous oxidation reaction (Jiang et al, 2014 ; Tang et al, 2016 ). Therefore, the adsorption energy for O 2 and CO on transition metals doped graphene is first calculated and the alternative decorating atom is chosen based on this rule.…”

Section: Introductionmentioning

confidence: 99%

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First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene

Jiang

Zhang

et al. 2018

Front. Chem.

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The CO oxidation mechanism on graphene with divacancy (DG) embedded with transition metal from Sc to Zn has been studied by using first principles calculations. The results indicate that O2 molecule is preferentially adsorbed on Sc, Ti, V, Cr, Mn, and Fe-DG, which can avoid the CO poisoning problem that many catalysts facing and is beneficial to the CO oxidation progress. Further study indicates that Mn-DG shows the best catalytic properties for CO oxidation with consideration of both Langmuir-Hinshelwood (LH) and Eley-Rideal (ER) oxidation mechanisms. Along the ER mechanism, the reaction energy barrier for the first step (CO free + O2 pre-adsorbed → OOCO) is 0.96 eV. Along the LH mechanism, the energy barrier for the rate limiting step (CO adsorbed + O2 adsorbed → OOCO) is only 0.41 eV, indicating that the CO oxidation on Mn-DG will occur along LH mechanism. The Hirshfeld charge distributions of O2 and CO molecules is tuned by the embedded Mn atom, and the charge transfer from the embedded Mn atom to the adsorbed molecules plays an important role for the CO oxidation. The result shows that the Mn-embedded divacancy graphene is a noble-metal free and efficient catalyst for CO oxidation at low temperature.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene

Jiang

Zhang

et al. 2018

Front. Chem.

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“…The O-O bond in O 2 elongates, which facilitates the facile oxidation of CO, for which the activation of O 2 is often the rate-limiting step. Following this work, many theoretical predictions were made with different substitutional dopant metallic atoms, including Fe [52][53][54], Cu [55], Pt [56], Al [57][58][59], Zn [59], Co [59], Ni [59], Sn [60], Mo [61], Pd [62,63], W [64], Mn [65], and Cr [66], and including non-metallic ones such as Si [67,68], N [69], P [69,70], Ge [58], demonstrating that such graphene support atoms are excellent thermocatalysts for CO oxidation, where the catalytic centers are at the dopants. By no means is this list exhaustive.…”

Section: Vacancy Enhanced Graphene Reactivitymentioning

confidence: 99%

Graphene-Based Heterogeneous Catalysis: Role of Graphene

et al. 2020

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Graphene, the reincarnation of a surface, offers new opportunities in catalytic applications, not only because of its peculiar electronic structure, but also because of the ease of modulating it. A vast number of proposals have been made to support this point, but there has been a lack of a systematic understanding of the different roles of graphene, as many other reviews published have focused on the synthesis and characterization of the various graphene-based catalysts. In this review, we surveyed the vast literature related to various theoretical proposals and experimental realizations of graphene-based catalysts to first classify and then elucidate the different roles played by graphene in solid-state heterogeneous catalysis. Owing to its one-atom thickness and zero bandgap with low density of states around Fermi level, graphene has great potential in catalysis applications. In general, graphene can function as a support for catalysts, a cover to protect catalysts, or the catalytic center itself. Understanding these functions is important in the design of catalysts in terms of how to optimize the electronic structure of the active sites for particular applications, a few case studies of which will be presented for each role.

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“…The single atom morphology and atomic coordination were identified by aberration‐corrected scanning transmission electron microscopy as well as STM . The charge transfer between metal atoms and graphene layer could effectively alter the chemical properties of the atoms, thereby promoting the molecular adsorption and catalytic reactions …”

Section: Single Carbon Vacanciesmentioning

confidence: 99%

“…[29] The charge transfer between metal atoms and graphene layer could effectively alter the chemical properties of the atoms, thereby promoting the molecular adsorption and catalytic reactions. [30]…”

Section: Single Carbon Vacanciesmentioning

confidence: 99%

Scanning Probe Microscopy of Topological Structure Induced Electronic States of Graphene

Liu

Qiu

2020

Small Methods

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Graphene, as the first emerging 2D material, has attracted considerable attention because of its remarkable physical properties and potential applications in future electronic devices. Due to its planar structure and monoatomic thickness, graphene is susceptible to the presence of structural and topological defects in lattices, which can have a pronounced influence on the electrical, optical, thermal, and magnetic properties of this carbon allotrope. To unravel the structural disorders at the atomic scale, characterization techniques such as scanning tunneling microscopy (STM) and atomic force microscopy (AFM) have been widely employed. These techniques enable atomically resolved visualization of the lattice imperfection in graphene, as well as a simultaneous interrogation of the electronic states associated with the structural perturbations. This short review highlights the recent advances in the application of STM and AFM for investigating various defects in graphene, including vacancies, substitutional dopants, non‐hexagonal rings, 1D homo‐ and hetero‐boundaries, and stacking misorientation and faults at interlayers. The understanding of the intrinsic properties of structural and topological defects in graphene is essential for developing graphene‐based functional materials and related devices.

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High catalytic activity for CO oxidation on single Fe atom stabilized in graphene vacancies

Abstract: The geometric, electronic and catalytic characters of Fe atom embedded graphene (including monovacancy and divacancy) are investigated using the first-principles method, which gives a reference on designing graphene-based catalysts for CO oxidation.

Cited by 65 publications

References 93 publications

First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene

First Principles Study on the CO Oxidation on Mn-Embedded Divacancy Graphene

Graphene-Based Heterogeneous Catalysis: Role of Graphene

Scanning Probe Microscopy of Topological Structure Induced Electronic States of Graphene

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